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Topotactic Transformation of Metal–Organic Frameworks to Graphene-Encapsulated Transition-Metal Nitrides as Efficient Fenton-like Catalysts
Open accessAbstract
Innovation in transition-metal nitride (TMN) preparation is highly desired for realization of various functionalities. Herein, series of graphene-encapsulated TMNs (Fe x Mn 6– x Co 4 –N@C) with well-controlled morphology have been synthesized through topotactic transformation of metal–organic frameworks in an N 2 atmosphere. The as-synthesized Fe x Mn 6– x Co 4 –N@C nanodices were systematically characterized and functionalized as Fenton-like catalysts for catalytic bisphenol A (BPA) oxidation by activation of peroxymonosulfate (PMS). The catalytic performance of Fe x Mn 6– x Co 4 –N@C was found to be largely enhanced with increasing Mn content. Theoretical calculations illustrated that the dramatically reduced adsorption energy and facilitated electron transfer for PMS activation catalyzed by Mn 4 N are the main factors for the excellent activity. Both sulfate and hydroxyl radicals were identified during the PMS activation, and the BPA degradation pathway mainly through hydroxylation, oxidation, and decarboxylation was investigated. Based on the systematic characterization of the catalyst before and after the reaction, the overall PMS activation mechanism over Fe x Mn 6– x Co 4 –N@C was proposed. This study details the insights into versatile TMNs for sustainable remediation by activation of PMS.
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Cites
Self-interaction correction to density-functional approximations for many-electron systems
Perdew, J. P., & Zunger, A. (1981) · Physical Review B · doi:10.1103/physrevb.23.5048 · Cited by 20,887
Cited by
Metal-Free Carbocatalysis in Advanced Oxidation Reactions
Duan, X., Sun, H., & Wang, S. (2018) · Accounts of Chemical Research · doi:10.1021/acs.accounts.7b00535 · Cited by 1,329
Self-citationAn, S., Zhang, G., Wang, T., Zhang, W., Li, K., Song, C., Miller, J. T., Miao, S., Wang, J., & Guo, X. (2018) · ACS Nano · doi:10.1021/acsnano.8b04693 · Cited by 601
Self-citationLim, J., Yang, Y., & Hoffmann, M. R. (2019) · Environmental Science & Technology · doi:10.1021/acs.est.9b01449 · Cited by 404
Metadata
- Authors
- Li, X., Ao, Z., Liu, J., Sun, H., Rykov, A. I., & Wang, J.
- Venue
- ACS Nano
- Publisher
- American Chemical Society (ACS)
- Published
- 2016-12-13
- Volume
- 10
- Issue
- 12
- Pages
- 11532-11540
- ISSN
- 1936-0851 (ISSN-L)
- 1936-086X
- OpenAlex
- W2560463761
- Cited by
- 309
- References
- 1
- FWCI
- 15.43
- Type
- journal article
- Language
- en
- Open access
- green
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- Li, X., Ao, Z., Liu, J., Sun, H., Rykov, A. I., & Wang, J. (2016). Topotactic Transformation of Metal–Organic Frameworks to Graphene-Encapsulated Transition-Metal Nitrides as Efficient Fenton-like Catalysts. ACS Nano. https://doi.org/10.1021/acsnano.6b07522
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